A model study for ambient air quality analysis using routine meteorological observations

In the present study, more realistic and easily adaptable input parameters have been used with a view to investigating the long-range air quality analysis for the dispersion of air pollutants emitted from an area source with a multiple box model. The model formulation has been discussed at length for the ground level sources when convective conditions prevail. The routine meteorological observations have been used for the computation of sensible surface heat flux, friction velocity and mixing depth. A radiation model provides the estimates of the sensible surface heat flux. Based on the similarity theory, an iterative procedure has been adopted for the estimation of friction velocity which provides a coupling of radiation computation and the surface layer of the planetary boundary layer through surface heat flux expression. The important parameters—wind speed and eddy diffusivity profiles—have been derived and have been used to obtain the concentration patterns as hourly averages. The procedure could be easily adopted where observed meteorological parameters may be used for studying the dispersal of pollutants from the ground level sources.     

Comparison between the atmospheric boundary layer in Paris and its rural suburbs during the ECLAP experiment

The ECLAP experiment has been performed during the winter of 1995 in order to study the influence of the urban area of Paris on the vertical structure and diurnal evolution of the atmospheric boundary layer, in situations favourable to intense urban heat island and pollution increase. One urban site and one rural site have been instrumented with sodars, lidars and surface measurements. Additional radiosondes, 100 m masts and Eiffel Tower data were also collected. This paper gives a general overview of this experiment, and presents results of the analysis of four selected days, characterized by various wind directions and temperature inversion strengths. This analysis, which consists in a comparison between data obtained in the two sites, has been focused on three parameters of importance to the ABL dynamics: the standard deviation of vertical velocity, the surface sensible heat flux, and the boundary layer height. The vertical component of turbulence is shown to be enhanced by the urban area, the amplitude of this effect strongly depending on the meteorological situation. The sensible heat flux in Paris is generally found larger than in the rural suburbs. The most frequent differences range from 25–65 W m^-2, corresponding to relative differences of 20–60%. The difference of unstable boundary layer height between both sites are most of the time less than 100 m. However, sodar and temperature data show that the urban influence is enhanced during night-time and transitions between stable and unstable regimes.     

Analysis of the influence of urban form and materials on sensible heat flux — a case study of Japan's largest housing development “Tama New Town”

In this study, the relationship between the form and materials of urban blocks and sensible heat flux from total surfaces was analyzed in the case of `Tama New Town', which is one of the largest housing developments in Japan and is under continuing development. First, urban blocks were divided into five categories depending on the building plot types. The characteristics of the form and thermal properties of each building, as well as the land cover condition (area of vegetation, bare soil, asphalt pavement, and built area) of each category was considered. Furthermore, 6 urban blocks were selected for numerical simulation of heat balance of the total surfaces, and sensible heat flux from the total surfaces of each urban block on clear sky summer day was calculated. It was confirmed that the influence of the direction that buildings faced and floor area ratio was as great as that of building materials upon the amount of sensible heat flux in each urban block.     

Ultrafine particle fluxes above four major European cities

Little information is known about the behaviour of ultrafine particles (UFP) on a citywide scale. Total particle number flux, dominated by UFP, and other meteorological parameters were collected from tower sites in Manchester, London, Edinburgh and Gothenburg between 1999 and 2006 using the eddy covariance technique. Averaged diurnal cycles were produced for particle number flux, concentration, sensible heat flux, emission velocity, friction velocity, wind speed and temperature. UFP flux cycles showed clear diurnal trends which were linked to traffic activity and local sources. Wind sector analysis showed contributions to flux from local heavily urbanised areas. A simple parameterised model linking UFP flux to traffic activity, sensible heat and friction velocity above the city was produced.     

Impact of anthropogenic heat on urban climate in Tokyo

This study quantifies the contribution through energy consumption, to the heat island phenomena and discussed how reductions in energy consumption could mitigate impacts on the urban thermal environment. Very detailed maps of anthropogenic heat in Tokyo were drawn with data from energy statistics and a very detailed digital geographic land use data set including the number of stories of building at each grid point. Animated computer graphics of the annual and diurnal variability in Tokyo's anthropogenic heat were also prepared with the same data sources. These outputs characterize scenarios of anthropogenic heat emission and can be applied to a numerical simulation model of the local climate. The anthropogenic heat flux in central Tokyo exceeded 400 W m⁻² in daytime, and the maximum value was 1590 W m⁻² in winter. The hot water supply in offices and hotels contributed 51% of this 1590 W m⁻². The anthropogenic heat flux from the household sector in the suburbs reached about 30 W m⁻² at night. Numerical simulations of urban climate in Tokyo were performed by referring to these maps. A heat island appeared evident in winter because of weakness of the sea breeze from Tokyo Bay. At 8 p.m., several peaks of high-temperature appeared, around Otemachi, Shinjuku and Ikebukuro; the areas with the largest anthropogenic heat fluxes. In summer the shortwave radiation was strong and the influence of anthropogenic heat was relatively small. In winter, on the other hand, the shortwave radiation was weak and the influence of anthropogenic heat was relatively large. The effects of reducing energy consumption, by 50% for hot water supply and 100% for space cooling, on near surface air temperature would be at most −0.5°C.     

Marble weathering and air pollution in Philadelphia

Maps of damage to marble tombstones in the urban region of Philadelphia demonstrate a close spatial correspondence with airborne pollutant concentrations. Mean recession rates on upper tombstone faces are an order of magnitude greater (3.5 mm (100a)⁻¹) in the center of the city than they are 20 km away in the suburbs and countryside (< 0.5 mm (100a)⁻¹). Not only are more pollutants emitted in the city, but they are also concentrated in the city center by centripetal air movement into the urban heat island. Gaseous SO₂ appears to be the most damaging pollutant, as is shown by the presence of gypsum in urban stones. Although rainfall is important in removing sulfate reaction products, anthropogenically-induced acid rain has only a minor role in marble deterioration. High urban SO₂ concentrations cause sufficient gypsum accumulation within the stones to exfoliate the durable surface layer. Old photos of tombstones in central Philadelphia cemeteries show that exfoliation greatly accelerated between 1930 and 1960, concurrent with increases in SO₂ levels. Recent improvements in air quality are likely to have slowed stone deterioration.     

Chemical transport models

Background, aim, and scope  Improving the parameterization of processes in the atmospheric boundary layer (ABL) and surface layer, in air quality and chemical transport models. To do so, an asymmetrical, convective, non-local scheme, with varying upward mixing rates is combined with the non-local, turbulent, kinetic energy scheme for vertical diffusion (COM). For designing it, a function depending on the dimensionless height to the power four in the ABL is suggested, which is empirically derived. Also, we suggested a new method for calculating the in-canopy resistance for dry deposition over a vegetated surface. Materials and methods  The upward mixing rate forming the surface layer is parameterized using the sensible heat flux and the friction and convective velocities. Upward mixing rates varying with height are scaled with an amount of turbulent kinetic energy in layer, while the downward mixing rates are derived from mass conservation. The vertical eddy diffusivity is parameterized using the mean turbulent velocity scale that is obtained by the vertical integration within the ABL. In-canopy resistance is calculated by integration of inverse turbulent transfer coefficient inside the canopy from the effective ground roughness length to the canopy source height and, further, from its the canopy height. Results  This combination of schemes provides a less rapid mass transport out of surface layer into other layers, during convective and non-convective periods, than other local and non-local schemes parameterizing mixing processes in the ABL. The suggested method for calculating the in-canopy resistance for calculating the dry deposition over a vegetated surface differs remarkably from the commonly used one, particularly over forest vegetation. Discussion  In this paper, we studied the performance of a non-local, turbulent, kinetic energy scheme for vertical diffusion combined with a non-local, convective mixing scheme with varying upward mixing in the atmospheric boundary layer (COM) and its impact on the concentration of pollutants calculated with chemical and air-quality models. In addition, this scheme was also compared with a commonly used, local, eddy-diffusivity scheme. Simulated concentrations of NO₂ by the COM scheme and new parameterization of the in-canopy resistance are closer to the observations when compared to those obtained from using the local eddy-diffusivity scheme. Conclusions  Concentrations calculated with the COM scheme and new parameterization of in-canopy resistance, are in general higher and closer to the observations than those obtained by the local, eddy-diffusivity scheme (on the order of 15–22%). Recommendations and perspectives  To examine the performance of the scheme, simulated and measured concentrations of a pollutant (NO₂) were compared for the years 1999 and 2002. The comparison was made for the entire domain used in simulations performed by the chemical European Monitoring and Evaluation Program Unified model (version UNI-ACID, rv2.0) where schemes were incorporated.     

Boundary-layer dynamics and its influence on atmospheric chemistry at Summit,Greenland

Sonic anemometer turbulence measurements were made at Summit, Greenland during summer 2004 and spring 2005. These measurements allow for the characterization of the variability of the atmospheric boundary layer at this site by describing seasonal and diurnal changes in sensible heat flux and boundary layer stability as well as providing estimates of mixing layer height. Diurnal sensible heat fluxes at Summit ranged from −18 to −2 W m⁻² in the spring and from −7 to +10 W m⁻² in the summer. Sustained stable surface layer conditions and low wind speeds occured during the spring but not during the summer months. Unstable conditions were not observed at Summit until late April. Diurnal cycles of convective conditions during the daytime (0700–1700 h local time) were observed throughout July and August. Boundary layer heights, which were estimated for neutral to stable conditions, averaged 156 m for the spring 2005 observations. Comparisons of the boundary layer characteristics of Summit with those from South Pole, Antarctica, provide possible explanations for the significant differences in snowpack and surface-layer chemistry between the two sites.     

Dry deposition and foliar leaching of mercury and selected trace elements in deciduous forest throughfall

The estimated annual throughfall deposition flux of Hg in a northern mixed-hardwood forest in the Lake Huron Watershed was 10.5±1.0 μg m⁻² compared to an annual precipitation Hg flux of 8.7±0.5 μg m⁻² (June 1996–June 1997). The source of this additional Hg in throughfall is often attributed to wash-off of dry deposition, but foliar leaching of Hg may also be important. To determine the influence of both dry deposition and foliar leaching of Hg and other elements in throughfall, we measured a suite of trace elements (Hg, Al, Mg, V, Mn, Cu, Zn, As, Rb, Sr, Cd, Ba, La, Ce, and Pb) in throughfall, precipitation, and ambient air samples from a northern mixed-hardwood forest. Based on a multiple linear regression model, dry deposition had the most important influence on Hg, Al, La, Ce, V, As, Cu, Zn, Cd, and Pb fluxes while foliar leaching strongly influenced Mg, Mn, Rb, Sr, and Ba fluxes in net throughfall. The Hg dry deposition flux was estimated using gaseous and aerosol Hg measurements and modeled deposition velocities. The calculated dry deposition flux (∼12–14 μg m⁻²) of Hg to the canopy indicated that atmospheric deposition of Hg could easily account for all of the Hg deposited in net throughfall (1.9±0.1 μg m⁻²). Although there is a large uncertainty associated with these techniques, the modeling estimates indicate that atmospheric Hg may account for all of the Hg deposited in litterfall (11.4±2.8 μg m⁻²).     

Dry deposition fluxes and deposition velocities of PAHs at an urban site in Turkey

Even though dry deposition and air–water exchange of semivolatile organic compounds (SOCs) are important for surfaces in and around the urban areas, there is still no generally accepted direct measurement technique for dry deposition. In this study, a modified water surface sampler (WSS) configuration, including a filter holder and an XAD-2 resin column, was employed to investigate the polycyclic aromatic hydrocarbon (PAH) dry deposition in an urban area. The measured total (particle+dissolved) PAH fluxes to the WSS averaged to be 34 960±16 540 ng m⁻² d⁻¹. Average particulate PAH flux, determined by analyzing the filter in the WSS, was about 8% of the total PAH flux. Temporal flux variations indicated that colder months (October–April) had the highest PAH fluxes. This increase could be attributed to the residential heating as well as meteorological effects including lower mixing height. A high volume air sampler was concurrently employed to collect ambient air concentrations. The average total (gas+particle) atmospheric PAH concentration (456±524 ng m⁻³) was within the range of previously measured values at different urban locations. PAH concentrations in urban areas are more than two orders of magnitude higher than those measured in pristine areas and this result may indicate that urban areas have major source sectors and greater deposition rates are expected near to these areas. The average contribution of particle phase was about 10% in total concentration. Simultaneous particulate phase dry deposition and ambient air samples were collected in this study. Then, particulate phase apparent dry deposition velocities were calculated using the fluxes and concentrations for each PAH compound and they ranged from 0.1 to 1.2 cm s⁻¹. These values are in good agreement with previously reported values.     

Ozone production from Grenoble city during the August 2003 heat wave

The heat wave from 1 to 16 August 2003 is considered in the city of Grenoble (French Alps). The modelling system (PREVALP) is based on several models operating on nested domains: MM5 for dynamics, CHIMERE for chemistry (18 km and 6 km grid size) and METPHOMOD for both dynamics and chemistry (2 km grid size). The analysis of the results shows that during the heat wave, the mixing layer is thicker, up to 3500 m agl, hence inducing transport of ozone to high altitude. Two regimes were diagnosed: (1) a freely developing convective layer, (2) a layer trapped under south wind which makes ozone precursors accumulate in the city. Local ozone production is estimated to be 40% of the plume maximum in case (2) and only 30% in case (1). Sensitivity analysis by step increase for temperature at the boundary of the inner domain shows the non-linearity of the response; in this case most of the effect comes from chemistry. By changing biogenic emission significant changes are observed in restricted areas.     

Elevational patterns of sulfur deposition at a site in the Catskill Mountains,New York

In this paper we report measurements of SO^2-₄ fluxes in throughfall and bulk deposition across an elevational transect from 800 to 1275 m on Slide Mountain in the Catskill Mountains of southeastern New York State. The net throughfall flux of SO^2-₄ (throughfall-bulk deposition), which we attribute to cloud and dry deposition, increased by roughly a factor of 13 across this elevational range. Part of the observed increase results from the year-round exposure of evergreen foliage at the high-elevation sites, compared to the lack of foliage in the dormant season in the deciduous canopies at low elevations. Comparison of the net throughfall flux with estimates of cloud deposition suggests that both cloud deposition and dry deposition increased with elevation. Dry deposition estimates from a nearby monitoring site fall within the measured range of net throughfall flux for SO^2-₄. The between-site variation in net throughfall flux was very high at the high-elevation sites, and less so at the lower sites, suggesting that studies of atmospheric deposition at high-elevations will be complicated by extreme spatial variability in deposition rates. Studies of atmospheric deposition in mountainous areas of the eastern U.S. have often emphasized cloud water deposition, but these results suggest that elevational increases in dry deposition may also be important.     

Determination of the latent heat flux in fog

The latent heat flux has been determined during a fog situation by using a method based on the surface heat balance equation and a parameterization of the sensible heat flux. The computed values of the latent heat flux show that it is connected with changes in fog density.     

Comparison of annual dry and wet deposition fluxes of selected pesticides in Strasbourg, France

This work summarizes the results of a study of atmospheric wet and dry deposition fluxes of Deisopropyl-atrazine (DEA), Desethyl-atrazine (DET), Atrazine, Terbuthylazine, Alachlor, Metolachlor, Diflufenican, Fenoxaprop-p-ethyl, Iprodione, Isoproturon and Cymoxanil pesticides conducted in Strasbourg, France, from August 2000 through August 2001. The primary objective of this work was to calculate the total atmospheric pesticide deposition fluxes induced by atmospheric particles. To do this, a modified one-dimensional cloud water deposition model was used. All precipitation and deposition samples were collected at an urban forested park environment setting away from any direct point pesticide sources. The obtained deposition fluxes induced by atmospheric particles over a forested area showed that the dry deposition flux strongly contributes to the total deposition flux. The dry particle deposition fluxes are shown to contribute from 4% (DET) to 60% (cymoxanil) to the total deposition flux (wet + dry).     

Growing season total gaseous mercury (TGM) flux measurements over an Acer rubrum L. stand

Relaxed eddy accumulation (REA) measurements of the total gaseous mercury (TGM) flux measurements were taken over a deciduous forest predominantly composed of Red Maple (Acer rubrum L.) during the growing season of 2004 and the second half of the growing season of 2005. The magnitudes of the flux estimates were in the range of published results from other micrometeorological mercury fluxes taken above a tall canopy and larger than estimates from flux chambers. The magnitude and direction of the flux were not static during the growing season. There was a significant trend (p < 0.001), from net deposition of TGM in early summer to net evasion in the late summer and early fall before complete senescence. A growing season atmosphere-canopy total mercury (TGM) compensation point during unstable daytime conditions was estimated at background ambient concentrations (1.41 ng m^?3). The trend in the seasonal net TGM flux indicates that long term dry deposition monitoring is needed to accurately estimate mercury loading over a forest ecosystem.     

Évaluation des propriétés énergétiques et microphysiques d'une source de convection artificielle à partir d' une étude de combustion organisée de fuel-oil en milieu naturel

To evaluate the potential environmental impacts of waste heat released by future dry cooling towers, an oil burning system which emits sensible heat at a rate of the order of 1000 MW into the atmosphere has been built up at the Centre de Recherches Atmosphériques. The project involved development of an oil burner device and experiments to quantify the amounts of heat and other matters released from oil combustion, such as gas and aerosol, that are not present in the case of cooling towers but may interact with heat and cause complications.The burner produces a flame of 3–5 m in height and 0.5–1.5 m in diameter. Fuel is consumed at a rate of 3.5–16.5 ℓ min⁻¹ at a pressure of 30–60 bars to develop a thermal output of 3–11 MW. The thermal power is distributed into three parts: sensible heat (82%), radiative energy (7–13%) and forced convection energy ( ~ 6 %); the two latter energy forms also heat the ambient air and so increase the real sensible heat output which eventually reaches 90 % of the thermal power.When the plume rises to some tens of meters, the combustion gas density is not very different from the air density and the additional water vapor does not exceed 5 % of the ambient water vapor.Smoke aerosol produced at the rate of 2–6gkg⁻¹ of fuel-oil exhibits a maximum concentration of 10⁷ particles cm⁻³ with a mean diameter of 0.5μm. The aerosol consists essentially of hydrophobic carbon (97%), while other elements, that may form hygroscopic or ice nuclei are present only in trace concentrations. The gaseous sulfur content may be higher but the SO₂ oxidation rate is very slow and then the cloud condensation nuclei amounts injected by the plume are neglegible in comparison with the natural nuclei. Thus the thermal impact on the atmosphere of the fuel oil combustion is essentially due to its thermodynamic characteristics, and our 105-burner system (Météotron) should correctly simulate in full scale a dry cooling tower. The smoke particles are quite useful as they make the plume visible and are used as passive tracers of the thermal disturbance.     

Development of a nonlocal convective mixing scheme with varying upward mixing rates for use in air quality and chemical transport models

BACKGROUND, AIM, AND SCOPE: Asymmetrical convective non-local scheme (CON) with varying upward mixing rates is developed for simulation of vertical turbulent mixing in the convective boundary layer in air quality and chemical transport models. MATERIALS AND METHODS: The upward mixing rate form the surface layer is parameterized using the sensible heat flux and the friction and convective velocities. Upward mixing rates varying with height are scaled with an amount of turbulent kinetic energy in layer, while the downward mixing rates are derived from mass conservation. RESULTS: This scheme provides a less rapid mass transport out of surface layer into other layers than other asymmetrical convective mixing schemes. DISCUSSION: In this paper, we studied the performance of a nonlocal convective mixing scheme with varying upward mixing in the atmospheric boundary layer and its impact on the concentration of pollutants calculated with chemical and air-quality models. This scheme was additionally compared versus a local eddy-diffusivity scheme (KSC). Simulated concentrations of NO(2) and the nitrate wet deposition by the CON scheme are closer to the observations when compared to those obtained from using the KSC scheme. CONCLUSIONS: Concentrations calculated with the CON scheme are in general higher and closer to the observations than those obtained by the KSC scheme (of the order of 15-20%). Nitrate wet deposition calculated with the CON scheme are in general higher and closer to the observations than those obtained by the KSC scheme. RECOMMENDATIONS AND PERSPECTIVES: To examine the performance of the scheme, simulated and measured concentrations of a pollutant (NO(2)) and nitrate wet deposition was compared for the year 2002. The comparison was made for the whole domain used in simulations performed by the chemical European Monitoring and Evaluation Programme Unified model (version UNI-ACID, rv2.0) where schemes were incorporated.     

Error estimations of dry deposition velocities of air pollutants using bulk sea surface temperature under common assumptions

It is well known that skin sea surface temperature (SSST) is different from bulk sea surface temperature (BSST) by a few tenths of a degree Celsius. However, the extent of the error associated with dry deposition (or uptake) estimation by using BSST is not well known. This study tries to conduct such an evaluation using the on-board observation data over the South China Sea in the summers of 2004 and 2006. It was found that when a warm layer occurred, the deposition velocities using BSST were underestimated within the range of 0.8–4.3%, and the absorbed sea surface heat flux was overestimated by 21 W m^?2. In contrast, under cool skin only conditions, the deposition velocities using BSST were overestimated within the range of 0.5–2.0%, varying with pollutants and the absorbed sea surface heat flux was underestimated also by 21 W m^?2. Scale analysis shows that for a slightly soluble gas (e.g., NO₂, NO and CO), the error in the solubility estimation using BSST is the major source of the error in dry deposition estimation. For a highly soluble gas (e.g., SO₂), the error in the estimation of turbulent heat fluxes and, consequently, aerodynamic resistance and gas-phase film resistance using BSST is the major source of the total error. In contrast, for a medium soluble gas (e.g., O₃ and CO₂) both the errors from the estimations of the solubility and aerodynamic resistance are important. In addition, deposition estimations using various assumptions are discussed. The largest uncertainty is from the parameterizations for chemical enhancement factors. Other important areas of uncertainty include: (1) various parameterizations for gas-transfer velocity; (2) neutral-atmosphere assumption; (3) using BSST as SST, and (4) constant pH value assumption.     

Rapid urban growth,land-use changes and air pollution in Santiago,Chile

This paper is a contribution to the understanding of the topoclimatic and environmental geography of the basin where Santiago — one of the most polluted Latin American city – is located. In the first part, land-use change is analysed looking at the climatic transformation caused by the rapid transit from natural semiarid surface to urban areas. In the second part, seasonal weather and daily cycles of slope winds and the available ventilation are described trying to relate those patterns with the spatial distribution of air pollution. A combination of meteorological, geographical and cultural factors explain extreme air pollution events: meteorologically, Santiago is under permanent subsidence inversion layers. Geographically, the city is located in a closed basin surrounded by mountains. Culturally, the urban area has the highest population concentration (40% of the national total), industries (near 70% of the total) and vehicles, which are the main sources of smog. The urban and suburban transport system is based on a large number of buses (diesel) and private cars, both experiencing a rapid growth from the past few years. The city and specially the transport system generates high emissions of pollutant, but the natural semiarid deforested soils and slopes are also important sources. The local wind system can explain the differential spatial distribution on the concentration of air pollutants in the city and its periphery. In winter (rain season) concentrations of particulate matter are higher at the centre and the SW part of the city. The andean piedmont area (E part of the city) shows minimum values, suggesting major ventilation effects of slope and valley winds. Ozone exceeds air quality standards in summer (dry season) at all sites in the centre and periphery. However, the O₃-concentrations are higher on preferred residential areas located at the piedmont area (E part of the city), suggesting air pollution transport effects. Currently, there is no consideration of these local climatic features in the process of urban planning.     

Numerical modeling of dry deposition coupled to 22 photochemical reactions

Three Eulerian models for the dry deposition of photochemically reactive species were formulated and evaluated: a K-theory model with independent transport and deposition of each species, a K-theory model coupled with 22 gas-phase reactions, and a second-order flux-budget model coupled with 22 reactions. Operator splitting was used to separately solve the reaction and dispersion terms in the models including photochemistry. In an evaluation of numerical method performance, the Adams–Moulton method with a pseudo-steady-state approximation for the free radicals was found to be consistent with, but more computationally efficient than Gear’s method for the solution of the reaction terms. The sensitivity of profiles of vertical concentration and flux to the Eulerian model formulation varied according to the species’ Damköhler number. Although a K-theory model is adequate for weakly depositing species with Damköhler numbers <10^-3, a second-order flux-budget model is required for species with Damköhler numbers that exceed unity, such as nitrogen oxides, free radicals, and those sensitive to net flux production by chemical reactions. Selection of an appropriate model formulation for the entire system depended on the most reactive species. Simple K-theory models may not accurately predict dry deposition fluxes in the urban surface layer.