Evaluating the ability of a numerical weather prediction model to forecast tracer concentrations during ETEX 2

In this paper the meteorological processes responsible for transporting tracer during the second ETEX (European Tracer EXperiment) release are determined using the UK Met Office Unified Model (UM). The UM predicted distribution of tracer is also compared with observations from the ETEX campaign. The dominant meteorological process is a warm conveyor belt which transports large amounts of tracer away from the surface up to a height of 4 km over a 36 h period. Convection is also an important process, transporting tracer to heights of up to 8 km. Potential sources of error when using an operational numerical weather prediction model to forecast air quality are also investigated. These potential sources of error include model dynamics, model resolution and model physics. In the UM a semi-Lagrangian monotonic advection scheme is used with cubic polynomial interpolation. This can predict unrealistic negative values of tracer which are subsequently set to zero, and hence results in an overprediction of tracer concentrations. In order to conserve mass in the UM tracer simulations it was necessary to include a flux corrected transport method. Model resolution can also affect the accuracy of predicted tracer distributions. Low resolution simulations (50 km grid length) were unable to resolve a change in wind direction observed during ETEX 2, this led to an error in the transport direction and hence an error in tracer distribution. High resolution simulations (12 km grid length) captured the change in wind direction and hence produced a tracer distribution that compared better with the observations. The representation of convective mixing was found to have a large effect on the vertical transport of tracer. Turning off the convective mixing parameterisation in the UM significantly reduced the vertical transport of tracer. Finally, air quality forecasts were found to be sensitive to the timing of synoptic scale features. Errors in the position of the cold front relative to the tracer release location of only 1 h resulted in changes in the predicted tracer concentrations that were of the same order of magnitude as the absolute tracer concentrations.     

Three long-range transport models compared to the ETEX experiment: a performance study

For operational or research purposes (dispersion computations of radioactive effluents during nuclear emergency situations, simulations of chemical pollution in the vicinity of thermal power plants), different models of passive dispersion in the atmosphere have been developed at the Environment Department of EDF’s R and D Division. This report presents the comparison of the performances of three such models: DIFTRA (lagrangian puff model, with operational goal), DIFEUL (three dimensional eulerian) and DIFPAR (Monte Carlo particle model) for the simulation of the first ETEX release, an international tracer campaign during which a passive tracer cloud has been followed over Europe. The results obtained in this study give model vs. experience differences of the same order as the model vs. experience differences observed during an international model comparison experiment using data of the Chernobyl release, the ATMES exercise. In addition to the standard statistical scores used in the evaluation of the performances of the transport models two asymmetric scores (in contradistinction with the Figure of Merit in Space) are proposed: “efficiency” and “power”. Their aim is to separate the two manners in which a model may be wrong: by predicting presence of pollutant while none is measured or conversely predicting absence when pollutant is actually detected.     

The field campaigns of the European Tracer Experiment (ETEX): overview and results

As part of the European Tracer Experiment (ETEX) two successful atmospheric experiments were carried out in October and November, 1994. Perfluorocarbon (PFC) tracers were released into the atmosphere in Monterfil, Brittany, and air samples were taken at 168 stations in 17 European countries for 72 h after the release. Upper air tracer measurements were made from three aircraft. During the first experiment a westerly air flow transported the tracer plume north-eastwards across Europe. During the second release the flow was eastwards. The results from the ground sampling network allowed the determination of the cloud evolution as far as Sweden, Poland and Bulgaria. This demonstrated that the PFT technique can be successfully applied in long-range tracer experiments up to 2000 km. Typical background concentrations of the tracer used are around 5–7 fl ?^-1 in ambient air. Concentrations in the plume ranged from 10 to above 200 fl/?^-1. The tracer release characteristics, the tracer concentrations at the ground and in upper air, the routine and additional meteorological observations at the ground level and in upper air, trajectories derived from constant-level balloons and the meteorological input fields for long-range transport models are assembled in the ETEX database. The ETEX database is accessible via the Internet. Here, an overview is given of the design of the experiment, the methods used and the data obtained.     

Comparison of constant volume balloons, model trajectories and tracer transport during ETEX

In the field phases of the European Tracer EXperiment (ETEX), an inert tracer was released for 12 h into the atmosphere and samples taken at several locations downwind. During the same time, several Constant Volume Balloons (CVB) (10 and 6 for ETEX first and second release, respectively) were launched into different altitudes and followed as far as 21–188 km, to indicate the initial dispersion directions of the tracer puff. A model simulating the CVB behaviour in hydrostatic meso-scale model forecasts is applied to ETEX data to demonstrate its capability to predict the tracer puff mean axis over long distances (−2000 km). CVB model results are first compared to air parcels trajectories and 2D (i.e. isentropic, isobaric and isodensity) trajectories. Then they are compared to the measured CVB trajectories and finally to the tracer puff trajectories. As expected, the CVB model and isodensity model trajectories are found to be identical. The 16 CVBs calculated trajectories nearly overlap the real ones over 21–188 km with mean absolute horizontal transport deviations less than 20 km (average value of 8.2 km). The corresponding relative transport deviations are less than 45% with an average value of 20.6%. Better predictions are obtained for the ETEX second release. During the 60 h following ETEX’s first release start, the simulated CVBs are mainly found in the area of the maximum surface concentrations of the released tracer, up to 2000 km. Up to 36 h after ETEX second tracer release start, the simulated CVB trajectories predict well the mean axis of the tracer puff, but failed later.     

Evaluation of the Meteo-France response in ETEX release 1

During ETEX Meteo-France applied part of its emergency response system for critical events developped in the framework of the World Meteorological Organization environmental emergency response program. The atmospheric transport model used to forecast the evolution of a passive tracer is an eulerian model called MEDIA. In real time this model is driven by meteorological data from ARPEGE, the operational numerical weather prediction model available at the Meteo-France operation center. The overall evaluation of the results show that the model can reproduce the cloud displacement, but there exists a stretching in the transport direction. In the ATMES-II phase, the results are closer to the observations when meteorological data from the European Center for Medium range Weather Forecast are used. A simulation using analyzed meteorological data from ARPEGE every 6 h slightly improve the results comparing with the real-time experiment. All the simulations we performed reveal that the quality of the atmospheric transport model is strongly dependent on the quality of the driving numerical weather prediction model.     

Validation of the UK Met. Office’s name model against the ETEX dataset

The ETEX 1 data set has been used to assess the performance of the UK Met Office’s long-range dispersion model NAME. In terms of emergency response modelling the model performed well, successfully predicting the overall spread and timing of the plume across Europe. However, in common with most other models, NAME overpredicted the observed concentrations. This is in contrast with other NAME validation studies which indicate either no significant bias or a tendency to underpredict concentrations. This suggests the reasons for overpredicting are specific to the ETEX situation. Explanations include inadequate vertical diffusion or transport, possible venting by convective activity, and experimental errors. An assessment of a range of advection schemes of varying complexity indicated no clear advantage, at present, in using more sophisticated random walk techniques at long range, a simple diffusion coefficient based scheme providing some of the best results. A brief look is also taken at a simulation of the more problematical ETEX 2 release.     

Tracer transport model at Japan meteorological agency and its application to the ETEX data

This paper describes the JMA tracer transport model and its sensitivity to model physics and initial conditions by using the ETEX data. Compared with observations, the model overestimates ground-level concentration in the early stage within about one day from the emission, possibly due to underestimation of vertical diffusion. In the early stage, the enhanced vertical diffusion effectively transports the tracer upward and decreases the ground-level concentration, while in the later stage, it enhances downward transports from the upper layer and increases the ground-level concentration. A conceptual model is given for understanding the vertical transport due to vertical diffusion. The horizontal diffusion introduced to the model has preferable impacts on forecasts especially in the early stage. Finally, we discuss the predictability of this model based on sensitivity to initial conditions of emission time and height.     

The use of weather radar in assessing deposition of radioactivity from chernobyl across England and Wales

Deposition of radionuclides from the Chernobyl accident depended critically on patterns of precipitation intercepting the material. This paper describes the use of the RAINPATCH model to calculate wet deposition of ¹³⁷Cs over England and Wales. This puff-based model makes direct use of precipitation data measured by weather radar to determine the scavenging of airborne material. The detailed spatial and temporal resolution of when and where material was scavenged provides good agreement with measurements. Since all the data used could potentially have been available at the time, such methods could usefully be applied in real time in the event of any future accident releasing such radionuclides.     

The chernobyl accident: Modelling of dispersion over europe of the radioactive plume and comparison with air activity measurements

Following the release of radionuclides from the Chernobyl power plant accident, a long-range transport and deposition model is used to describe the plume dispersion over Europe. The aim of this study is the validation of a fast Lagrangjan model and a better understanding of the relative impact of some mechanisms, such as the initial plume rise. Comparisons between results and ¹³⁷Cs measurement activity are discussed according to spatial and temporal variations. It is shown that many measurements can be explained only if the initial plume rise taken at 925, 850 and 700mb is considered.     

Validation of the lagrangian particle dispersion model FLEXPART against large-scale tracer experiment data

A comprehensive validation of FLEXPART, a recently developed Lagrangian particle dispersion model based on meteorological data from the European Centre for Medium-Range Weather Forecasts, is described in this paper. Measurement data from three large-scale tracer experiments, the Cross-Appalachian Tracer Experiment (CAPTEX), the Across North America Tracer Experiment (ANATEX) and the European Tracer Experiment (ETEX) are used for this purpose. The evaluation is based entirely on comparisons of model results and measurements paired in space and time. It is found that some of the statistical parameters often used for model validation are extremely sensitive to small measurement errors and should not be used in future studies. 40 cases of tracer dispersion are studied, allowing a validation of the model performance under a variety of different meteorological conditions. The model usually performs very well under undisturbed meteorological conditions, but it is less skilful in the presence of fronts. The two ETEX cases reveal the full range of the model’s skill, with the first one being among the best cases studied, and the second one being, by far, the worst. The model performance in terms of the statistical parameters used stays rather constant with time over the periods (up to 117 h) studied here. It is shown that the method used to estimate the concentrations at the receptor locations has a significant effect on the evaluation results. The vertical wind component sometimes has a large influence on the model results, but on the average only a slight improvement over simulations which neglect the vertical wind can be demonstrated. Subgrid variability of mixing heights is important and must be accounted for.     

Conceptual Design of a Massive Aerometric Tracer Experiment (MATEX)

A hypothetical field experiment is evaluated that relates, through tracer releases, reactive pollutant emissions to long range transport and deposition. The feasibility of such an approach is established provided certain requirements can be met. The experiment must: (a) trace emissions from several sources simultaneously and repetitively over an extended period of time, (b) link a tracer to the chemical behavior of emissions, and (c) apply a statistically sound method of guidance for deducing empirical source-receptor relationships (SRRs) while accounting for natural variability. One design approach would use perfluoro-carbon tracers (PFTs), which are nonreactive in the atmosphere, to simulate the transport and dispersion of reactive species such as sulfur and nitrogen oxides. Conversion and loss factors would be calibrated using isotopic sulfur and nitrogen compounds with PFTs, in combination with aerometric and deposition observations. An experimental concept is described that determines SRRs for deposition from observations and their interpolation, synthesized by an empirical model. If implemented, the experiment would be very expensive and has high design risk for achieving its goals given present knowledge.     

Ensemble-based data assimilation and targeted observation of a chemical tracer in a sea breeze model

We study the use of ensemble-based Kalman filtering of chemical observations for constraining forecast uncertainties and for selecting targeted observations. Using a coupled model of two-dimensional sea breeze dynamics and chemical tracer transport, we perform three numerical experiments. First, we investigate the chemical tracer forecast uncertainties associated with meteorological initial condition and forcing error. We find that the ensemble variance and error builds during the transition between land and sea breeze phases of the circulation. Second, we investigate the effects on the forecast variance and error of assimilating tracer concentration observations extracted from a truth simulation for a network of surface locations. We find that assimilation reduces the variance and error in both the observed variable (chemical tracer concentrations) and unobserved meteorological variables (vorticity and buoyancy). Finally, we investigate the potential value to the forecast of targeted observations. We calculate an observation impact factor that maximizes the total decrease in model uncertainty summed over all state variables. We find that locations of optimal targeted observations remain similar before and after assimilation of regular network observations.     

Using chemical models for evaluating the geochemical confinement capacity of a geological barrier application to the Centre de Stockage de l'Aube (France)

The feasibility of using a chemical reaction-based approach for evaluating and modelling the role of adsorption reactions in determining the geochernical confinement capacity of natural geological barriers is being studied as part of an on-going R & D programme. The confined superficial aquifer underlying the Centre de Stockage de l'Aube facility, a geological barrier for this site, has been used as a case study with the following aims. First, development of a site characterisation protocol and demonstration of its use to determine the principal geochemical characteristics of aquifer materials using batch experiments and to represent the information obtained in terms of a chemical model. The experimental results obtained for Ni²⁺ partitioning as a function of total Ni, pH, total Ca and total solid can be satisfactorily represented in terms of reactions with an ion exchange site and a single amphoteric surface hydroxyl site with ferrihydrite reaction constants. A second objective is the incorporation of the reactions in a coupled geochemistry/transport code, and to verify the applicability of the coupled code predictions for Ni²⁺ mass transfer by comparison with the results obtained during column tracer experiments. The breakthrough curve and equilibrium solid phase Ni loading, predicted by a one-dimensional coupled model for a column tracer experiment, agree closely with observed data.Additional studies are underway to reduce model conditionality, to extend the adsorption model to other analogue cations and anions, to incorporate the effect of natural organic matter and to take into consideration precipitation/dissolution of amorphous Fe surface phases.     

Sensitivity of the DERMA long-range Gaussian dispersion model to meteorological input and diffusion parameters

The Danish Emergency Response Model of the Atmosphere (DERMA) is described and applied to the first ETEX experiment. By using analysed low-resolution numerical weather-prediction data from the global model of the European Centre for Medium-range Weather Forecast (ECMWF) as well as higher-resolution data from two versions of the High Resolution Limited Area Model (HIRLAM), which are operational at the Danish Meteorological Institute (DMI), the sensitivity of DERMA to the resolution of meteorological data is analysed by comparing DERMA results with concentration measurements. Furthermore, the sensitivity to boundary-layer height and diffusion parameters is studied. These parameters include the critical bulk Richardson number, which is used to estimate the atmospheric boundary-layer height, the horizontal eddy diffusivity and the Lagrangian turbulence time scale. The parameters, which provide the best performance of DERMA, are 0.25 for the critical bulk Richardson number, 6×10³ m² s^-1 for the horizontal eddy diffusivity, and 3 h for the Lagrangian time scale. DERMA is much more sensitive to boundary-layer parameters when using high-resolution DMI-HIRLAM data than when using data of lower resolution from the ECMWF. Finally, the bulk Richardson number method of boundary-layer height calculation applied to DMI-HIRLAM data is verified directly against routine radiosondes released under the tracer gas plume. The boundary-layer height estimates based on analysed NWP model data agree well with observations, and the agreement deteriorates as a function of forecast length.     

Norwegian Meteorological Institute’s real-time dispersion model snap (Severe Nuclear Accident Program): Runs for ETEX and ATMES II experiments with different meteorological input

The Norwegian Meteorological Institute (DNMI) has developed and implemented for operational use a real-time dispersion model Severe Nuclear Accident Program (SNAP) with capability for predicting concentrations and depositions of the radioactive debris from large accidental releases. SNAP has been closely linked to DNMI’s operational numerical weather prediction (NWP) models.How good are these predictions? Participation in ETEX has partly answered this question. DNMI used SNAP with LAM50S giving meteorological input for these real-time dispersion calculations. LAM50S Limited Area Model with 50 km grid squareswas DNMI’s operational NWP model in 1994 when ETEX took place.In this article we report on how SNAP performed in the first of the ETEX releases in near-real-time mode, using LAM50S—and in hindcast mode for ATMES II, using “ECMWF 1995: ETEX Data set (ATMES II)”as meteorological input data. These two input data sets came from NWP models with quite different characteristics but with similar resolution in time and space.The results from these dispersion simulations matched closely. Deviations early in the simulation period shrank to insignificant differences later on. Since both input data sets were based on “weather analysis” and had similar resolution in space and time, SNAP described the dispersion of the released material very similar in these two simulations.     

Source function estimate by means of variational data assimilation applied to the ETEX-I tracer experiment

The ETEX data set opens new possibilities to develop data assimilation procedures in the area of long-range transport. This paper illustrates the possibilities using a variational approach, where the source term for ETEX-I was reconstructed. The MATCH model (Robertson et al., 1996) has been the basis for this attempt. The timing of the derived emission rates are in accordance with the time period for the ETEX-I release, and a cross validation, with observations beyond the selected assimilation period, shows that the source term gained holds for the entire ETEX-I experiment. A poor-man variational approach was shown to perform nearly as good as a fully variational data assimilation. The issue of quality control has not been considered in this attempt but will be an important part that has to be addressed in future work.     

Concentrations and fluxes of organic compounds in the atmosphere of the Swedish west coast

Measurements of organic compounds in air and deposition have been carried out in parallel on the Swedish west coast. In this investigation the importance of long-range transport for the occurrence of organic compounds in deposition has been studied. Air samples were collected using a high volume sampler (HVS) and the deposition was sampled on a 1 m² Teflon-coated horizontal surface with runoff for the precipitation to an adsorbent. The samples were analyzed in order to identify and quantify different semivolatile compounds such as PAH and petrogenic hydrocarbons and chlorinated compounds such as PCB, HCH and HCB. Qualitative differences between the content of organic compounds in air and deposition during periods with varying levels of air pollution and different meteorological conditions have been studied and a comparison with other air pollutants, such as soot, has been carried out. The results of the measurements show that deposition of PAH and other hydrocarbons takes place continuously but the greatest amounts are measured in the deposition in connection with episodes together with heavy precipitation. The highest concentrations of PCB and HCH in the air were obtained during a warm dry period in May and the greatest amounts were deposited in a period in May with heavy precipitation.     

Development of a regional oxidant model and application to the northeastern United States

Elevated oxidant concentrations due to the long-range transport of ozone and its precursors have been observed in many rural areas in the continental United States. The oxidation processes associated with ozone formation in the atmosphere have many important implications for regional air quality problems, such as regional haze and acid deposition. This paper describes the development and evaluation of a mesoscale photochemical air quality simulation model (RTM-III) covering the northeastern United States. The model considers an area 2080 km in the E-W direction by 1840 km in the N-S direction, with a spatial resolution on the order of 80 x 80 km, and a temporal resolution on the order of one hour. Data collected during an episode in July 1978 by the EPRI Sulfate Regional Experiment is used for testing and evaluating the model. In a comparison of hourly predictions with observations, the model predictions, with a few exceptions where local influences are suspected, generally track the measured spatial pattern and diurnal variation of ozone concentrations quite well. The correlation coefficient matched by time and location over more than 1500 pairs of hourly predicted and observed ozone concentrations is 0.7.     

Atmospheric mercury species in the European Arctic: Measurements and modelling

Concentrations of different species of mercury in arctic air and precipitation have been measured at Ny-Ålesund (Svalbard) and Pallas (Finland) during 1996–1997. Typical concentrations for vapour phase mercury measured at the two stations were in the range of 0.7–2 ng m⁻³ whereas particulate mercury concentrations were below 5 pg m⁻³. Total mercury in precipitation was in the range 3–30 ng l⁻¹. In order to evaluate the transport and deposition of mercury to the arctic from European anthropogenic sources, the Eulerian transport model HMET has been modified and extended to also include mercury species. A scheme for chemical conversion of elemental mercury to other species of mercury and deposition characteristics of different mercury species have been included in the model. European emission inventories for three different forms of Hg (Hg⁰, HgCl₂ and Hg_p) have been implemented in the numerical grid system for the HMET model.     

The impact of transpacific transport of mineral dust in the United States

We use a global chemical transport model (GEOS-Chem) to estimate the impact of transpacific transport of mineral dust on aerosol concentrations in North America during 2001. We have implemented two dust mobilization schemes in the model (GOCART and DEAD) and find that the best simulation of North American surface observations with GEOS-Chem is achieved by combining the topographic source used in GOCART with the entrainment scheme used in DEAD. This combination restricts dust emissions to year-round arid areas but includes a significant wind threshold for dust mobilization. The model captures the magnitude and seasonal cycle of observed surface dust concentrations over the northern Pacific. It simulates the free tropospheric outflow of dust from Asia observed in the TRACE-P and ACE-Asia aircraft campaigns of spring 2001. It reproduces the timing and distribution of Asian dust outbreaks in North America during April–May. Beyond these outbreaks we find persistent Asian fine dust (averaging 1.2 μg m⁻³) in surface air over the western United States in spring, with much weaker influence (0.25 μg m⁻³) in summer and fall. Asian influence over the eastern United States is 30–50% lower. We find that transpacific sources accounted for 41% of the worst dust days in the western United States in 2001.