A trajectory plume model for simulating air pollution transients

An air quality simulation model that is simple, yet capable of accurately estimating concentrations under unsteady meteorological conditions, has been developed. This trajectory plume model uses the Gaussian plume equation, but has an applicability that is approximately as wide as the Lagrangian puff model. The plume axis is represented by a series of straight-line plume segments. The performance of this model was evaluated by comparing it with other diffusion models. A comparison between simulation results using the present model and those using integrated puff and Eulerian diffusion models for three different metropolitan areas (one in Japan and two in the U.S.) has indicated that a simple trajectory plume model performs as well as the two other more complex models in simulating pollutant dispersion under complicated meteorological conditions such as those which occur during the transition period from a sea breeze to a land breeze.     

Evaluation of dynamic subgrid-scale models in large-eddy simulations of neutral turbulent flow over a two-dimensional sinusoidal hill

Large-eddy simulation (LES) is used to simulate neutral turbulent boundary-layer flow over a rough two-dimensional sinusoidal hill. Three different subgrid-scale (SGS) models are tested: (a) the standard Smagorinsky model with a wall-matching function, (b) the Lagrangian dynamic model, and (c) the recently developed scale-dependent Lagrangian dynamic model [Stoll, R., Porté-Agel, F., 2006. Dynamic subgrid-scale models for momentum and scalar fluxes in large-eddy simulation of neutrally stratified atmospheric boundary layers over heterogeneous terrain. Water Resources Research 42, W01409. doi:10.1029/2005WR003989]. The simulation results obtained with the different models are compared with turbulence statistics obtained from experiments conducted in the meteorological wind tunnel of the AES (Atmospheric Environment Service, Canada) [Gong, W., Taylor, P.A., Dörnbrack, A., 1996. Turbulent boundary-layer flow over fixed aerodynamically rough two-dimensional sinusoidal waves. Journal of Fluid Mechanics 312, 1–37]. We find that the scale-dependent dynamic model is able to account, without any tuning, for the local changes in the eddy-viscosity model coefficient. It can also capture the scale dependence of the coefficient associated with regions of the flow with strong mean shear and flow anisotropy. As a result, the scale-dependent dynamic model yields results that are more realistic than the ones obtained with the scale-invariant Lagrangian dynamic model.     

Comparison of a new Eulerian model with a modified Lagrangian approach for particle distribution and deposition indoors

Understanding of aerosol dispersion characteristics has many scientific and engineering applications. It is recognized that Eulerian or Lagrangian approach has its own merits and limitations. A new Eulerian model has been developed and it adopts a simplified drift–flux methodology in which external forces can be incorporated straightforwardly. A new near-wall treatment is applied to take into account the anisotropic turbulence for the modified Lagrangian model. In the present work, we present and compare both Eulerian and Lagrangian models to simulate particle dispersion in a small chamber. Results reveal that the standard k–ε Lagrangian model over-predicts particle deposition compared to the present turbulence-corrected Lagrangian approach. Prediction by the Eulerian model agrees well with the modified Lagrangian model.     

Description of sorbing tracers transport in fractured media using the lattice model approach

The transport of contaminants in fractured media is a complex phenomenon with a great environmental impact. It has been described with several models, most of them based on complex partial differential equations, that are difficult to apply when equilibrium and nonequilibrium dynamics are considered in complex boundaries. With the aim of overcoming this limitation, a combination of two lattice Bathnagar, Gross and Krook (BGK) models, derived from the lattice Boltzmann model, is proposed in this paper. The fractured medium is assumed to be a single fissure in a porous rock matrix. The proposed approach permits us to deal with two processes with different length scales: advection–dispersion in the fissure and diffusion within the rock matrix. In addition to the mentioned phenomena, sorption reactions are also considered. The combined model has been tested using the experimental breakthrough curves obtained by Garnier et al. (Garnier, J.M., Crampon, N., Préaux, C., Porel, G., Vreulx, M., 1985. Traçage par ¹³C, ²H, I⁻ et uranine dans la nappe de la craie sénonienne en écoulement radial convergent (Béthune, France). J. Hidrol. 78, 379–392.) giving acceptable results. A study on the influence of the lattice BGK models parameters controlling sorption and matrix diffusion on the breakthrough curves shape is included.     

A lagrangian dispersion model for calculating concentration distribution within a built-up domain

A Lagrangian model to study the dispersion of pollutants between urban buildings is described. The flow field is supplied by an objective analysis (Rockle (1990) Ph.D. thesis, Vom Fachbereich Mechanik, der Technischen Hochschule Darmstadt, Germany) and is adjusted to satisfy the continuity equation. From the resulting; mass consistent field the Lagrangian diffusion parameters are eliminated. A 3-D Lagrangian diffusion model in a nonhomogeneous field is applied to calculate the pollutant distribution between the buildings. Several examples are studied and compared to wind tunnel measurements.     

The relation between ozone,NOx and hydrocarbons in urban and polluted rural environments

Research over the past ten years has created a more detailed and coherent view of the relation between O₃ and its major anthropogenic precursors, volatile organic compounds (VOC) and oxides of nitrogen (NO_x). This article presents a review of insights derived from photochemical models and field measurements. The ozone–precursor relationship can be understood in terms of a fundamental split into a NO_x-senstive and VOC-sensitive (or NO_x-saturated) chemical regimes. These regimes are associated with the chemistry of odd hydrogen radicals and appear in different forms in studies of urbanized regions, power plant plumes and the remote troposphere. Factors that affect the split into NO_x-sensitive and VOC-sensitive chemistry include: VOC/NO_x ratios, VOC reactivity, biogenic hydrocarbons, photochemical aging, and rates of meteorological dispersion. Analyses of ozone–NO_x–VOC sensitivity from 3D photochemical models show a consistent pattern, but predictions for the impact of reduced NO_x and VOC in indivdual locations are often very uncertain. This uncertainty can be identified by comparing predictions from different model scenarios that reflect uncertainties in meteorology, anthropogenic and biogenic emissions. Several observation-based approaches have been proposed that seek to evaluate ozone–NO_x–VOC sensitivity directly from ambient measurements (including ambient VOC, reactive nitrogen, and peroxides). Observation-based approaches have also been used to evaluate emission rates, ozone production efficiency, and removal rates of chemically active species. Use of these methods in combination with models can significantly reduce the uncertainty associated with model predictions.     

Non-linear response of wet deposition to emissions reduction: A model study

An Eulerian atmospheric model with complex chemistry (Acidic Deposition and Oxidant Model) and a Lagrangian model with linear chemistry (Ontario Ministry of the Environment Trajectory Model) were used to simulate the wet SO₄²⁻ deposition pattern over eastern North America for 16 days during April 1981.The two model results agree reasonably well with each other when the 16 day average values are compared. They also show reasonable agreement with observed data. Having established the ability of the models to predict deposition patterns for 1981 emissions, reduction scenarios with 50% SO_x and 50% SO_x and NO_x of the 1981 emissions were studied through the Eulerian model. Near the heavy emissions area, the reduction in SO₄²⁻ wet deposition is only about 30–40%. In this respect the linear Lagrangian model departs significantly from the Eulerian model. This non-linearity in response is attributed to the role of oxidants in controlling the conversion of SO₂ to SO₄²⁻.     

A comparison of chemical mechanisms based on TRAMP-2006 field data

A comparison of a model using five widely known mechanisms (RACM, CB05, LaRC, SAPRC-99, SAPRC-07, and MCMv3.1) has been conducted based on the TexAQS II Radical and Aerosol Measurement Project (TRAMP-2006) field data in 2006. The concentrations of hydroxyl (OH) and hydroperoxy (HO₂) radicals were calculated by a zero-dimensional box model with each mechanism and then compared with the OH and HO₂ measurements. The OH and HO₂ calculated by the model with different mechanisms show similarities and differences with each other and with the measurements. First, measured OH and HO₂ are generally greater than modeled for all mechanisms, with the median modeled-to-measured ratios ranging from about 0.8 (CB05) to about 0.6 (SAPRC-99). These differences indicate that either measurement errors, the effects of unmeasured species or chemistry errors in the model or the mechanisms, with some errors being independent of the mechanism used. Second, the modeled and measured ratios of HO₂/OH agree when NO is about 1 ppbv, but the modeled ratio is too high when NO was less and too low when NO is more, as seen in previous studies. Third, mechanism–mechanism HO_x differences are sensitive to the environmental conditions – in more polluted conditions, the mechanism–mechanism differences are less. This result suggests that, in polluted conditions, the mechanistic details are less important than in cleaner conditions, probably because of the dominance of reactive nitrogen chemistry under polluted conditions.     

Description of sorbing tracers transport in fractured media using the lattice model approach

The transport of contaminants in fractured media is a complex phenomenon with a great environmental impact. It has been described with several models, most of them based on complex partial differential equations, that are difficult to apply when equilibrium and nonequilibrium dynamics are considered in complex boundaries. With the aim of overcoming this limitation, a combination of two lattice Bathnagar, Gross and Krook (BGK) models, derived from the lattice Boltzmann model, is proposed in this paper. The fractured medium is assumed to be a single fissure in a porous rock matrix. The proposed approach permits us to deal with two processes with different length scales: advection-dispersion in the fissure and diffusion within the rock matrix. In addition to the mentioned phenomena, sorption reactions are also considered. The combined model has been tested using the experimental breakthrough curves obtained by Garnier et al. (Garnier, J.M., Crampon, N., Préaux, C., Porel, G., Vreulx, M., 1985. Tra?age par 13C, 2H, I- et uranine dans la nappe de la craie sénonienne en écoulement radial convergent (Béthune, France). J. Hidrol. 78, 379-392.) giving acceptable results. A study on the influence of the lattice BGK models parameters controlling sorption and matrix diffusion on the breakthrough curves shape is included.     

Fully coupled “online” chemistry within the WRF model

A fully coupled “online” Weather Research and Forecasting/Chemistry (WRF/Chem) model has been developed. The air quality component of the model is fully consistent with the meteorological component; both components use the same transport scheme (mass and scalar preserving), the same grid (horizontal and vertical components), and the same physics schemes for subgrid-scale transport. The components also use the same timestep, hence no temporal interpolation is needed. The chemistry package consists of dry deposition (“flux-resistance” method), biogenic emission as in [Simpson et al., 1995. Journal of Geophysical Research 100D, 22875–22890; Guenther et al., 1994. Atmospheric Environment 28, 1197–1210], the chemical mechanism from RADM2, a complex photolysis scheme (Madronich scheme coupled with hydrometeors), and a state of the art aerosol module (MADE/SORGAM aerosol parameterization).The WRF/Chem model is statistically evaluated and compared to MM5/Chem and to detailed photochemical data collected during the summer 2002 NEAQS field study. It is shown that the WRF/Chem model is statistically better skilled in forecasting O₃ than MM5/Chem, with no appreciable differences between models in terms of bias with the observations. Furthermore, the WRF/Chem model consistently exhibits better skill at forecasting the O₃ precursors CO and NO_y at all of the surface sites. However, the WRF/Chem model biases of these precursors and of other gas-phase species are persistently higher than for MM5/Chem, and are most often biased high compared to observations. Finally, we show that the impact of other basic model assumptions on these same statistics can be much larger than the differences caused by model differences. An example showing the sensitivity of various statistical measures with respect to the treatment of biogenic volatile organic compounds emissions illustrates this impact.     

Dynamic-chemical coupling of the upper troposphere and lower stratosphere region

The importance of the interaction between chemistry and dynamics in the upper troposphere and lower stratosphere for chemical species like ozone is investigated using two chemistry-climate models and a Lagrangian trajectory model. Air parcels from the upper troposphere, i.e. regions of lightning and aircraft emissions, are able to be transported into the lowermost stratosphere (LMS). Trajectory calculations suggest that the main transport pathway runs via the inter tropical convergence zone, across the tropical tropopause and then to higher latitudes, i.e. into the LMS. NOx from aircraft emissions at mid-latitudes are unlikely to perturb the LMS since they are washed-out while still in the troposphere. In contrast, NOx from tropical lightning has the chance to accumulate in the LMS. Because of the longer residence times of NOx in the LMS, compared to the upper troposphere, this excess NOx from lightning has the potential to form ozone in the LMS, which then is transported back to the troposphere at mid-latitudes. In the models, around 10% of the ozone concentration and 50% of the NOx concentration in the northern hemisphere LMS is produced by lightning NOx At least 5% of the ozone concentration and 35% the NOx concentration at 150 hPa at mid-latitudes originates from tropical lightning in the climate-chemistry simulations.     

Diffusion of an instantaneous cluster of particles in homogeneous turbulence

In this work we study the diffusion of instantaneous puffs vs the diffusion of continuous plumes. The model which we use is a Lagrangian model for the motion of N particles suggested by Kaplan and Dinar (1988, J. compt. Phys. 79, 317–335). This model is based on the approach of Richardson to the relative diffusion which states that the instantaneous relative velocity of particles is a function of their instantaneous separation. Results show that the diffusion of a puff is slower than that of a continuous source. We find that the puff evolves more slowly than in the analytic model of Lee and Stone (1983, Atmospheric Environment17, 2477–2481), since in their model diffusion is influenced only by the initial conditions. The effect of the source size on the diffusion rate is studied as well.     

Numerical simulation of scalar dispersion downstream of a square obstacle using gradient-transport type models

We present a numerical study of scalar transport released from a line source downstream of a square obstacle to investigate the capabilities and limitations of gradient-transport modeling in predicting atmospheric dispersion. The standard k–? and k–ω models and a Reynolds Stress Transport closure are employed and compared to predict the time-averaged turbulent flow field, while a standard gradient–diffusion model is initially adopted to relate the scalar flux to mean gradients of the concentration field. The analysis of two algebraic closures for turbulent scalar fluxes based on the generalized-gradient–diffusion hypothesis and its quadratic extension is also presented. In spite of the rather simple flow setup, where both the flow and the scalar fields can be assumed homogeneous in the spanwise direction, the analysis clarifies several critical issues concerning gradient-transport type models. We established the dominant role of predicted turbulent kinetic energy on scalar dispersion when a scalar diffusivity is employed, irrespectively of the Reynolds stress closure adopted for the averaged momentum equation. Moreover, the standard gradient–diffusion hypothesis failed to predict the streamwise component of the scalar flux, which is characterized by a counter-gradient-transport mechanism. Although the resulting contribution in the averaged scalar transport equation is small in the present flow configuration, this limitation can become severe for strongly inhomogeneous flows in the presence of point sources, where the spread of the scalar plume is essentially three-dimensional. The predictive capabilities of gradient-transport type modeling are found clearly improved using algebraic closures, which appear to represent a promising tool for predicting atmospheric dispersion in complex flows when unsteady transport mechanisms are not dominant.     

Simulation of short-range diffusion experiment in low-wind convective conditions

A previously obtained analytical solution to model the short-range dispersion of pollutants in low winds from surface releases has been used to simulate diffusion tests conducted during winter in weakly convective conditions at the Indian Institute of Technology (IIT) Delhi. The turbulence parameterization based on friction velocity has been tested to simulate diffusion experiment. Such a parameterization in this study is considered justifiable on two counts: (1) prevailing meteorological and dispersion conditions have been generally of weakly unstable type as indicated by values of Monin–Obukhov length and bulk Richardson number, (2) uncertainties associated with the application of convective velocity based similarity parameterization to simulation of diffusion experiment at IIT Delhi, resulting in significant underprediction in most of the cases (Atmos. Environ. 30 (1996a) 1137). With this parameterization, the model simulations have improved considerably and compare reasonably well with the observations. Further, the results from a simple Gaussian model have been included for comparison. This study is in continuation of the work done earlier to simulate near-source dispersion in weak winds.     

A Lagrangian stochastic model for predicting concentration fluctuations in urban areas

A combined Lagrangian stochastic model with a micromixing sub-model is used to estimate the fluctuating concentrations observed in two wind tunnel experiments. The Lagrangian stochastic model allows fluid trajectories to be simulated in the inhomogeneous flow, while the mixing model accounts for the dissipation of fluctuations using the interaction by exchange with the mean (IEM) mechanism. The model is first tested against the open terrain, wind tunnel data of Fackrell, J.E. and Robins, A.E. [1982. Concentration fluctuations and fluxes in plumes from point sources in a turbulent boundary layer. Journal of Fluid Mechanics 117, 1–26] and shows good agreement with the observed mean concentrations and fluctuation intensities. The model is then compared with the wind tunnel simulation of a two-dimensional street canyon by Pavageau, M. and Schatzmann, M. [1999. Wind tunnel measurements of concentration fluctuations in an urban street canyon. Atmospheric Environment 33, 3961–3971]. Despite the limitations of the k–ε turbulence scheme and the IEM mixing mechanism, the model reproduces the fluctuation intensity pattern within the canyon well. Overall, the comparison with both sets of wind tunnel experiments are encouraging, and the simplicity of the model means that predictions in a complex, three-dimensional geometry can be produced in a practicable amount of time.     

Chemistry and aerosols in the marine boundary layer: 1-D modelling of the three ACE-2 Lagrangian experiments

Three Lagrangian experiments were conducted during IGAC's second aerosol characterization experiment (ACE-2) in the area between Portugal, Tenerife and Madeira in June/July 1997. During each Lagrangian experiment, a boundary layer air mass was followed for about 30 h, and the temporal evolution of its chemical and aerosol composition was documented by a series of vertical profiles and horizontal box pattern flown by the Meteorological Research Flight research aircraft Hercules C130. The wealth of observational data that has been collected during these three Lagrangian experiments is the basis for the development and testing of a one-dimensional Lagrangian boundary layer model with coupled gas, aqueous, and aerosol phase chemistry. The focus of this paper is on current model limitations and strengths. We show that the model is able to represent the dynamical and chemical evolution of the marine boundary layer, in some cases requiring adjustments of the subsidence velocity and of the surface heat fluxes. Entrainment of a layer rich in ozone and carbon monoxide from a residual continental boundary layer into the marine boundary layer as well as in-cloud oxidation of sulphur dioxide by hydrogen peroxide are simulated, and coherent results are obtained, concerning the evolution of the small, presumably sulphate–ammonia aerosol mode.     

Erratum to “Continuous four-dimensional source attribution for the Berlin area during two days in July 1994. Part I: The new Euler–Lagrange-model system LaMM5”: [Atmospheric Environment 35 (32) (2001) 5497]

The multiple nested three-dimensional (3D) mesoscale Eulerian grid point model MM5 was directly coupled with a Lagrangian particle trajectory model in order to perform a 4D source attribution for the area of Berlin based on the import probability density (IPD) distribution of the according receptor box. Within the resulting model system LaMM5 introduced here, the IPD distributions are not based on backward trajectories, which lack the recognition of the turbulent environment, but on the forward integration of a huge amount (order of million per day) of particle releases according to an emission scenario which is approximately continuous in space and time. Hence, the receptor import yields an accordingly continuous IPD distribution. Much attention has been paid on spatial and temporal resolution at the interface between both model parts (online-coupling) and the interface itself has been extended by the turbulent quantities resulting from the higher-order turbulence closure of the Eulerian model part. LaMM5 is applied on an episode with high photochemical activity across Berlin at two consecutive days (25 and 26 July 1994) with varying meteorological conditions leading to an accordingly different source attribution. The main results are:

• •The decay of the Berlin IPD with increasing source-receptor distance and time appears in an exponential manner if only sources out of a constant level (z=25 m) are regarded.
• •Heterogeneous wind fields in time and space enhance the contributions (emissions) of nearby sources to the total import of the receptor in contrast to stationary wind fields which increase the scope of the IPD distribution in upstream direction.

There are further results from several additional sensitivity studies presented in a companion paper B (Part II).     

An efficient Lagrangian stochastic model of vertical dispersion in the convective boundary layer

We consider the one-dimensional case of vertical dispersion in the convective boundary layer (CBL) assuming that the turbulence field is stationary and horizontally homogeneous. The dispersion process is simulated by following Lagrangian trajectories of many independent tracer particles in the turbulent flow field, leading to a prediction of the mean concentration. The particle acceleration is determined using a stochastic differential equation, assuming that the joint evolution of the particle velocity and position is a Markov process. The equation consists of a deterministic term and a random term. While the formulation is standard, attention has been focused in recent years on various ways of calculating the deterministic term using the well-mixed condition incorporating the Fokker–Planck equation. Here we propose a simple parameterisation for the deterministic acceleration term by approximating it as a quadratic function of velocity. Such a function is shown to represent well the acceleration under moderate velocity skewness conditions observed in the CBL. The coefficients in the quadratic form are determined in terms of given turbulence statistics by directly integrating the Fokker–Planck equation. An advantage of this approach is that, unlike in existing Lagrangian stochastic models for the CBL, the use of the turbulence statistics up to the fourth order can be made without assuming any predefined form for the probability distribution function (PDF) of the velocity. The main strength of the model, however, lies in its simplicity and computational efficiency. The dispersion results obtained from the new model are compared with existing laboratory data as well as with those obtained from a more complex Lagrangian model in which the deterministic acceleration term is based on a bi-Gaussian velocity PDF. The comparison shows that the new model performs well.     

Using a reduced Common Representative Intermediates (CRIv2-R5) mechanism to simulate tropospheric ozone in a 3-D Lagrangian chemistry transport model

A reduced chemical scheme (CRIv2-R5) which describes ozone formation from the tropospheric degradation of methane and 22 emitted non-methane hydrocarbons and oxygenated volatile organic compounds has been applied in a global-3D chemistry transport model (STOCHEM). The scheme, which contains 220 species in 609 reactions, has been used to simulate ozone and its precursors for the meteorological year of 1998 and the results have been compared with those from STOCHEM runs with its original chemistry. Compared with the original chemistry scheme, the degradation of a larger number of more reactive VOCs in the CRI scheme results in the formation (and their consequent transportation) of more NO_x active reservoirs thus leading to formation of more ozone away from land-based sources. Conversely, the more reactive VOCs also lead to greater removal of OH in continental areas and greater formation of OH in marine environments. STOCHEM run with the CRI scheme simulates more ozone (by up to 10 ppb), which results in better agreement with observed vertical ozone profiles. The CRI scheme transforms the globally and annually integrated ozone budget for the considered year in STOCHEM from a net loss of ?55 Tg yr^?1 to a net gain of +50 Tg yr^?1.